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Phil Kessel forced overtime for the Maple Leafs with his seventh of the season at 15:40 of the third.
Neal, Crosby, Beau Bennett and Pascal Dupuis scored in regulation for Pittsburgh (17-8-0), which outshot Toronto 41-26. Crosby scored in his first game in Toronto in over three years to extend his point streak to a season-high seven games (five goals, 10 assists).
"I thought we played a really good game," Crosby said. "I thought we did some really good things.
"It's a fun building, a fun atmosphere. We didn't want to let them get back into the game ... but they pushed hard and kept coming."
The Penguins won despite going 0-for-4 on the power play and allowing two man-advantage goals to Toronto in three opportunities.
"It was certainly a big factor in the game," Penguins coach Dan Bylsma said. "We get two power-play goals on us rather quickly in this game.
"It's definitely a big part of where we're at right now."
Crosby, who leads the NHL with 40 points (12 goals, 28 assists), played in Toronto for the first time since Jan. 9, 2010.
In 11 career visits, Crosby has nine goals and six assists. He has an eight-game point streak against the Maple Leafs.
Overall, Crosby has 19 goals and 19 assists in 24 career meetings with the Maple Leafs.
Pittsburgh outshot Toronto 13-5 in the first period and grabbed a quick lead when Neal scored his 16th of the season just 36 seconds in. Matt Niskanen's point shot was partially blocked, but the puck dribbled into the slot to Neal, who fired a shot past Reimer.
Van Riemsdyk tied it at 7:14 during a power play, scoring his 14th goal, but Crosby and Bennett combined to give Pittsburgh a 3-1 lead.
"We had a little bit of a slow start. We kind of got caught standing around and watching them a little too much," Phaneuf said. "We recognized that during the intermission and went after them.
"It was huge to come back and get that point but we definitely would've liked to have two."
Crosby netted his 12th goal at 14:31 after Reimer couldn't control Kris Letang's shot, allowing Letang to get the rebound back to Crosby. Bennett's shot got past Reimer at 15:21, giving Bennett his second of the season.
Franson's second of the year pulled Toronto within a goal on the power play at 10:12 of the second, while Crosby was off for tripping. Dupuis put Pittsburgh ahead 4-2 at 13:01 with his ninth, but MacArthur made it 4-3 a minute later with his seventh.
Reimer finished with 37 saves but lost for the first time in seven starts. He fought the puck early, and was eager to pull out a win in the shootout.
"There were a couple of goals I didn't want to have go in," he said. "When you can get to a shootout and get a point, you kind of have a chance to redeem yourself. That's when you want to step up and be big for your teammates.
"That wasn't the case and that's what I'm most frustrated about. We battled back hard enough as a team and I had a chance to be there for the boys and wasn't able to do it."
- Forward Matt Frattin returned to Toronto's lineup after missing 12 games because of a knee injury.
- Pittsburgh's Evgeni Malkin earned an assist on Bennett's goal, giving him points in nine of 11 games in Toronto.
- The Maple Leafs entered leading the NHL in hits (773) and fighting majors (25).
- The Penguins will be back in Toronto for another game on Thursday.
- Crosby came into the game with an average of 1.63 points per game, the NHL's best mark since Penguins owner Mario Lemieux averaged 1.77 points per game in the 2000-01 season.